The lead halide perovskites demonstrate huge potential for optoelectronic applications, high energy radiation detectors, light emitting devices and solar energy harvesting. Those materials exhibit strong spin-orbit coupling enabling efficient optical orientation of carrier spins in perovskite-based devices with performance controlled by a magnetic field. Here we show that elaborated time-resolved spectroscopy involving strong magnetic fields can be successfully used for perovskites. We perform a comprehensive study of high-quality lead halide perovskite CsPbBr3 crystals by measuring the exciton and charge carrier g-factors, spin relaxation times and hyperfine interaction of carrier and nuclear spins by means of coherent spin dynamics. Owing to their ‘inverted’ band structure, perovskites represent appealing model systems for semiconductor spintronics exploiting the valence band hole spins, while in conventional semiconductors the conduction band electrons are considered for spin functionality.
The original version of this Article contained an error in Fig. 2c, in which the numbers on the y-axis were given in the wrong order: '800' at the bottom through to '0' at the top. This has been corrected in both the PDF and HTML versions of the Article. Also, the Source Data file initially published online was corrupted and was replaced.
The spin structure and spin dynamics of excitons in an ensemble of (In,Al)As/AlAs quantum dots (QDs) with type-I band alignment, containing both direct and indirect band gap dots, are studied. Time-resolved and spectral selective techniques are used to distinguish between the direct and indirect QDs. The exciton fine structure is studied by means of optical alignment and optical orientation techniques in magnetic fields applied in the Faraday or Voigt geometries. A drastic difference in emission polarization is found for the excitons in the direct QDs involving a Γ-valley electron and the excitons in the indirect QDs contributed by an X-valley electron. We show that in the direct QDs the exciton spin dynamics is controlled by the anisotropic exchange splitting, while in the indirect QDs it is determined by the hyperfine interaction with nuclear field fluctuations. The anisotropic exchange splitting is determined for the direct QD excitons and compared with model calculations.c is the maximal circular polarization degree achieved in strong fields, µ B is the Bohr magneton, and g ex is the longitudinal exciton g-factor. The latter is composed of the Γ-electron (g e ) and heavy hole (g hh ) gfactors: g ex = g hh − g e . Both dependencies of ρ l (B) and
The exciton spin dynamics are investigated both experimentally and theoretically in twomonolayer-thick GaAs/AlAs quantum wells with an indirect band gap and a type-II band alignment. The magnetic-field-induced circular polarization of photoluminescence, Pc, is studied as function of the magnetic field strength and direction as well as sample temperature. The observed nonmonotonic behaviour of these functions is provided by the interplay of bright and dark exciton states contributing to the emission. To interpret the experiment, we have developed a kinetic master equation model which accounts for the dynamics of the spin states in this exciton quartet, radiative and nonradiative recombination processes, and redistribution of excitons between these states as result of spin relaxation. The model offers quantitative agreement with experiment and allows us to evaluate, for the studied structure, the heavy-hole g factor, g hh = +3.5, and the spin relaxation times of electron, τse = 33 µs, and hole, τ sh = 3 µs, bound in the exciton.
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